1) reset the content of the old cache by adding the following command in a batch file and running it (of course you can add the parameter in the registry manually, but it's quite handy to have the batch ready whenever you need to reset the cache):
REG ADD "HKLM\System\CurrentControlSet\Services\CSC\Parameters" /v FormatDatabase /t REG_DWORD /d 1 /f
2) Reboot, the added key will be detected, all the content of the cache will be deleted, as well as the key itself (it only resets once)
3) Add the following registry key in the same HKLM\System\CurrentControlSet\Services\CSC\Parameters section of the registry:
Type: REG SZ (string)
Name: CacheLocation
Value: the new location in NT format, ie \??\d:\csc if you want to create the new cache in d:\csc.

I entered \\??\C:\Users\UserID\Documents and rebooted. I then enabled offline files, rebooted and got the blue memory dump screen. I ended up having to restore from a System restore to get back to normal.

Are there different steps that I should take, or can I just not set the CSC location as Documents?

To redirect my documents on a per user basic you can do this: Go to the properties of my documents -> location tab -> define a new network location to redirect to, if necessary make that network folder available offline

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